Artificial photosynthesis for CO2-to-ethylene conversion enabled by dye-sensitised carbon nitrides

染料敏化碳氮化物实现人工光合作用将二氧化碳转化为乙烯

• 批准号: 2749474
• 金额: --
• 依托单位: University of Cambridge
• 依托单位国家: 英国
• 项目类别: Studentship
• 财政年份: 2022
• 资助国家: 英国
• 起止时间: 2022 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=studentship-2749474
• 关键词: Artificial; photosynthesis; CO2; ethylene; conversion

Photoelectrochemical (PEC) cells are unique devices combining direct solar light conversion into chemical bonds with the compactness and catalytic tuneability of electrolysis. Photoelectrocatalysis is a promising solution for the scalable synthesis of solar fuels, i.e. chemicals with deliverable energetic content, and photoreforming, that is the light-driven conversion of waste into added-value products. On the cathodic side, solar-driven CO2 reduction to hydrocarbons and other organic molecules is a promising venue to solar fuels synthesis and strategy for decarbonisation. For the anodic reaction, glycerol has been proposed as excellent photoreforming substrate for its facile oxidation and its current overproduction as a byproduct of the synthesis of biodiesel. However, glycerol oxidation usually leads to a mixture of products, including glyceraldehyde and 1,3-dihydroxyacetone, with the latter being more valuable. The purpose of this Ph.D. project will be to design and fabricate a stand-alone PEC device comprising a photocathode for high-rate synthesis of C2-C3 hydrocarbons from CO2 and a photoanode for the selective photoreforming of glycerol to 1,3-dihydroxyacetone in acidic environment. The incorporation of a tandem perovskite solar cell in a copper-based photocathode will enable conversion of CO2 to hydrocarbons at very positive onset potentials and record-breaking photocurrents. On the other hand, different light-absorbing semiconductors, including polymeric carbon nitrides and perovskites, will be screened for the fabrication of a photoanode for glycerol oxidation. Selectivity of the anodic reaction will be achieved either by state-of-the-art Pt-Bi electrocatalysts or substrate-specific enzymes. Finally, the two electrodes will be combined in a stand-alone device for a bias-free, solar-driven complete redox cycle.

光电化学(PEC)电池是一种独特的设备，它将太阳能直接转换为化学键与电解的紧凑性和催化可调性相结合。光电催化是一种很有前途的解决方案，可用于可规模合成太阳能燃料(即具有可提供的含能含量的化学品)和光重整(即通过光驱动将废物转化为附加值产品)。在阴极方面，太阳能驱动的二氧化碳还原为碳氢化合物和其他有机分子是太阳能燃料合成和脱碳策略的一个有希望的场所。对于阳极反应，甘油是一种很好的光转化底物，因为它容易氧化，目前作为生物柴油合成的副产物而产生过多。然而，甘油氧化通常会产生包括甘油醛和1，3-二羟基丙酮在内的混合产物，后者更有价值。本博士项目的目的是设计和制造一种独立的PEC器件，该器件包括用于从二氧化碳快速合成C2-C3烃的光阴极和用于甘油在酸性环境中选择性光重整合成1，3-二羟基丙酮的光阳极。在铜基光电阴极中引入串联钙钛矿太阳能电池将使二氧化碳在非常正的起始电位和创纪录的光电流下转化为碳氢化合物。另一方面，将筛选不同的吸光半导体，包括聚合物氮化碳和钙钛矿，以制备甘油氧化的光阳极。阳极反应的选择性将通过最先进的铂-铋电催化剂或底物特定的酶来实现。最后，这两个电极将被组合在一个独立的设备中，以实现无偏压、太阳能驱动的完整氧化还原循环。